Synthesis of pyrimidines from dinitrogen and carbon

Abstract

The element nitrogen and nitrogenous compounds are vital to life. The synthesis of nitrogen-containing compounds using dinitrogen as the nitrogen source, not through ammonia, is of great interest and great value but remains a grand challenge. Herein, we describe a strategy to realize this transformation by combining the heterogeneous approach with the homogeneous methodology. The N₂ molecule was first fixed with carbon and LiH through a one-pot heterogeneous process, forming Li₂CN₂ as an 'activated' nitrogen source with high efficiency. Then subsequent homogeneous treatments of Li₂CN₂ to construct the organic synthon carbodiimide and the RNA/DNA building block pyrimidines were fulfilled. By using ¹⁵N₂ as the feedstock, their corresponding ¹⁵N-labeled carbodiimide and pyrimidines were readily obtained. This homogeneous-heterogeneous synergy strategy will open a new chapter for N₂ transformation.

Keywords: 15n-labeled pyrimidines; N−C bond formation; dinitrogen transformation; homogeneous–heterogeneous synergy strategy; nitrogen fixation.